The transition of a Mott insulator to metal, the Mott transition, can occur via carrier doping by elemental substitution, and by photoirradiation, as observed in transition-metal compounds and in organic materials. Here, we show that the application of a strong electric field can induce a Mott transition by a new pathway, namely through impulsive dielectric breakdown. Irradiation of a terahertz electric-field pulse on an ET-based compound, κ-(ET) Cu[N(CN)]Br (ET:bis(ethylenedithio)tetrathiafulvalene), collapses the original Mott gap of ∼30 meV with a ∼0.1 ps time constant after doublon-holon pair productions by quantum tunnelling processes, as indicated by the nonlinear increase of Drude-like low-energy spectral weights. Additionally, we demonstrate metallization using this method is faster than that by a femtosecond laser-pulse irradiation and that the transition dynamics are more electronic and coherent. Thus, strong terahertz-pulse irradiation is an effective approach to achieve a purely electronic Mott transition, enhancing the understanding of its quantum nature.
A rapid polarization control in paraelectric materials is important for an ultrafast optical switching useful in the future optical communication. In this study, we applied terahertz-pump second-harmonic-generation-probe and optical-reflectivity-probe spectroscopies to the paraelectric neutral phase of an organic molecular dielectric, tetrathiafulvalene-p-chloranil and revealed that a terahertz pulse with the electric-field amplitude of ∼400 kV/cm produces in the subpicosecond time scale a large macroscopic polarization whose magnitude reaches ∼20% of that in the ferroelectric ionic phase. Such a large polarization generation is attributed to the intermolecular charge transfers and breathing motions of domain walls between microscopic neutral and ionic domains induced by the terahertz electric field.
Ultrafast photoinduced transitions of a one-dimensional Mott insulator into two distinct electronic phases, metal and charge-density-wave (CDW) state, were achieved in a bromine-bridged Pd-chain compound [Pd(en)2Br](C5-Y)2H2O (en=ethylenediamine and C5-Y=dialkylsulfosuccinate), by selecting the photon energy of a femtosecond excitation pulse. For the resonant excitation of the Mott-gap transition, excitonic states are generated and converted to one-dimensional CDW domains. For the higher-energy excitation, free electron and hole carriers are produced, giving rise to a transition of the Mott insulator to a metal. Such selectivity in photoconversions by the choice of initial photoexcited states opens a new possibility for the developments of advanced optical switching and memory functions.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.